Designing a Naturally Inspired Conductive Copolymer to Engineer Wearable Bioadhesives for Sensing Applications.

The design of adhesive and conductive soft hydrogels using biopolymers with tunable mechanical properties has received significant interest in the field of wearable sensors for detecting human motions. These hydrogels are primarily fabricated through the modification of biopolymers to introduce cross-linking sites, the conjugation of adhesive components, and the incorporation of conductive materials into the hydrogel network. The development of a multifunctional copolymer that integrates adhesive and conductive properties within a single polymer chain with suitable cross-linking sites eliminates the need for biopolymer modification and the addition of extra conductive and adhesive components. In this study, we synthesized a copolymer based on poly([2-(methacryloyloxy)ethyl] trimethylammonium chloride-co-dopamine methacrylamide) (p(METAC-DMA)) using a controlled radical polymerization, allowing for the efficient conjugation of both adhesive and conductive units within a single polymer chain. Subsequently, our multifunctional hydrogel named Gel-MD was fabricated by mixing the p(METAC-DMA) copolymer with non-modified gelatin in which cross-linking took place in an oxidative environment. We confirmed the biocompatibility of the Gel-MD hydrogel through in vitro studies using NIH 3T3 cells as well as in vivo subcutaneous implantation in rats. Furthermore, the Gel-MD hydrogel was effective and sensitive in detecting various human motions, making it a promising wearable sensor for health monitoring and diagnosis.

Particle morphology and soil properties affect the retention of copper oxide nanoparticles in agricultural soils.

The interaction between nanoscale copper oxides (nano-CuOs) and soil matrix significantly affects their fate and transport in soils. This study investigates the retention of nano-CuOs and Cu2+ ions in ten typical agricultural soils by employing the Freundlich adsorption model. Retention of nano-CuOs and Cu2+ in soils was well fitted by the Freundlich model. The retention parameters (KD, KF, and N) followed an order of CuO NTs > CuO NPs > Cu2+, highlighting significant impact of nano-CuOs morphology. The KF and N values of CuO NPs/Cu2+ were positively correlated with soil pH and electrical conductivity (EC), but exhibited a weaker correlation for CuO NTs. Soil pH and/or EC could be used to predict KF and N values of CuO NPs or CuO NTs, with additional clay content should be included for Cu2+.The different relationship between retention parameters and soil properties may suggest that CuO NTs retention mainly caused by agglomeration, whereas adsorption and agglomeration were of equal importance to CuO NPs. The amendment of Ca2+ at low and medium concentration promoted retention of nano-CuOs in alkaline soils, but reduced at high concentration. These findings provided critical insights into the fate of nano-CuOs in soil environments, with significant implications for environmental risk assessment and soil remediation strategies.

3D printable and biocompatible PEDOT:PSS-ionic liquid colloids with high conductivity for rapid on-demand fabrication of 3D bioelectronics.

3D printing has been widely used for on-demand prototyping of complex three-dimensional structures. In biomedical applications, PEDOT:PSS has emerged as a promising material in versatile bioelectronics due to its tissue-like mechanical properties and suitable electrical properties. However, previously developed PEDOT:PSS inks have not been able to fully utilize the advantages of commercial 3D printing due to its long post treatment times, difficulty in high aspect ratio printing, and low conductivity. We propose a one-shot strategy for the fabrication of PEDOT:PSS ink that is able to simultaneously achieve on-demand biocompatibility (no post treatment), structural integrity during 3D printing for tall three-dimensional structures, and high conductivity for rapid-prototyping. By using ionic liquid-facilitated PEDOT:PSS colloidal stacking induced by a centrifugal protocol, a viscoplastic PEDOT:PSS-ionic liquid colloidal (PILC) ink was developed. PILC inks exhibit high-aspect ratio vertical stacking, omnidirectional printability for generating suspended architectures, high conductivity (~286 S/cm), and high-resolution printing (~50 µm). We demonstrate the on-demand and versatile applicability of PILC inks through the fabrication of 3D circuit boards, on-skin physiological signal monitoring e-tattoos, and implantable bioelectronics (opto-electrocorticography recording, low voltage sciatic nerve stimulation and recording from deeper brain layers via 3D vertical spike arrays).

Conductive Hydrogel Tapes for Tripolar EEG: A Promising Solution to Paste-Related Challenges.

Electroencephalography (EEG) remains pivotal in neuroscience for its non-invasive exploration of brain activity, yet traditional electrodes are plagued with artifacts and the application of conductive paste poses practical challenges. Tripolar concentric ring electrode (TCRE) sensors used for EEG (tEEG) attenuate artifacts automatically, improving the signal quality. Hydrogel tapes offer a promising alternative to conductive paste, providing mess-free application and reliable electrode-skin contact in locations without hair. Since the electrodes of the TCRE sensors are only 1.0 mm apart, the impedance of the skin-to-electrode impedance-matching medium is critical. This study evaluates four hydrogel tapes' efficacies in EEG electrode application, comparing impedance and alpha wave characteristics. Healthy adult participants underwent tEEG recordings using different tapes. The results highlight varying impedances and successful alpha wave detection despite increased tape-induced impedance. MATLAB's EEGLab facilitated signal processing. This study underscores hydrogel tapes' potential as a convenient and effective alternative to traditional paste, enriching tEEG research methodologies. Two of the conductive hydrogel tapes had significantly higher alpha wave power than the other tapes, but were never significantly lower.

Changes of in vivo electrical conductivity in the brain and torso related to age, fat fraction and sex using MRI.

This work was inspired by the observation that a majority of MR-electrical properties tomography studies are based on direct comparisons with ex vivo measurements carried out on post-mortem samples in the 90's. As a result, the in vivo conductivity values obtained from MRI in the megahertz range in different types of tissues (brain, liver, tumors, muscles, etc.) found in the literature may not correspond to their ex vivo equivalent, which still serves as a reference for electromagnetic modelling. This study aims to pave the way for improving current databases since the definition of personalized electromagnetic models (e.g. for Specific Absorption Rate estimation) would benefit from better estimation. Seventeen healthy volunteers underwent MRI of both brain and thorax/abdomen using a three-dimensional ultrashort echo-time (UTE) sequence. We estimated conductivity (S/m) in several classes of macroscopic tissue using a customized reconstruction method from complex UTE images, and give general statistics for each of these regions (mean-median-standard deviation). These values are used to find possible correlations with biological parameters such as age, sex, body mass index and/or fat volume fraction, using linear regression analysis. In short, the collected in vivo values show significant deviations from the ex vivo values in conventional databases, and we show significant relationships with the latter parameters in certain organs for the first time, e.g. a decrease in brain conductivity with age.

Enhancing electrical conductivity and mechanical properties of decellularized umbilical cord arteries using graphene coatings.

Traditional decellularized bioscaffolds possessing intact vascular networks and unique architecture have been extensively studied as conduits for repairing nerve damage. However, they are limited by the absence of electrical conductivity, which is crucial for proper functioning of nervous tissue. This study focuses on investigating decellularized umbilical cord arteries by applying coatings of graphene oxide (GO) and reduced graphene oxide (RGO) to their inner surfaces. This resulted in a homogeneous GO coating that fully covered the internal lumen of the arteries. The results of electrical measurements demonstrated that the conductivity of the scaffolds could be significantly enhanced by incorporating RGO and GO conductive sheets. At a low frequency of 0.1 Hz, the electrical resistance level of the coated scaffolds decreased by 99.8% with RGO and 98.21% with GO, compared with uncoated scaffolds. Additionally, the mechanical properties of the arteries improved by 24.69% with GO and 32.9% with RGO after the decellularization process. The GO and RGO coatings did not compromise the adhesion of endothelial cells and promoted cell growth. The cytotoxicity tests revealed that cell survival rate increased over time with RGO, while it decreased with GO, indicating the time-dependent effect on the cytotoxicity of GO and RGO. Blood compatibility evaluations showed that graphene nanomaterials did not induce hemolysis but exhibited some tendency toward blood coagulation.

MXene-Based Flexible Electrodes for Electrophysiological Monitoring.

The advancement of flexible electrodes triggered research on wearables and health monitoring applications. Metal-based bioelectrodes encounter low mechanical strength and skin discomfort at the electrode-skin interface. Thus, recent research has focused on the development of flexible surface electrodes with low electrochemical resistance and high conductivity. This study investigated the development of a novel, flexible, surface electrode based on a MXene/polydimethylsiloxane (PDMS)/glycerol composite. MXenes offer the benefit of featuring highly conductive transition metals with metallic properties, including a group of carbides, nitrides, and carbonitrides, while PDMS exhibits inherent biostability, flexibility, and biocompatibility. Among the various MXene-based electrode compositions prepared in this work, those composed of 15% and 20% MXene content were further evaluated for their potential in electrophysiological sensing applications. The samples underwent a range of characterization techniques, including electrochemical impedance spectroscopy (EIS), cyclic voltammetry (CV), as well as mechanical and bio-signal sensing from the skin. The experimental findings indicated that the compositions demonstrated favorable bulk impedances of 280 and 111 Ω, along with conductivities of 0.462 and 1.533 mS/cm, respectively. Additionally, they displayed promising electrochemical stability, featuring charge storage densities of 0.665 mC/cm2 and 1.99 mC/cm2, respectively. By conducting mechanical tests, Young's moduli were determined to be 2.61 MPa and 2.18 MPa, respectively. The composite samples exhibited elongation of 139% and 144%, respectively. Thus, MXene-based bioelectrodes show promising potential for flexible and wearable electronics and bio-signal sensing applications.

Silver Nanowire-Based Flexible Strain Sensor for Human Motion Detection.

Accurately capturing human movements is a crucial element of health status monitoring and a necessary precondition for realizing future virtual reality/augmented reality applications. Flexible motion sensors with exceptional sensitivity are capable of detecting physical activities by converting them into resistance fluctuations. Silver nanowires (AgNWs) have become a preferred choice for the development of various types of sensors due to their outstanding electrical conductivity, transparency, and flexibility within polymer composites. Herein, we present the design and fabrication of a flexible strain sensor based on silver nanowires. Suitable substrate materials were selected, and the sensor's sensitivity and fatigue properties were characterized and tested, with the sensor maintaining reliability after 5000 deformation cycles. Different sensors were prepared by controlling the concentration of silver nanowires to achieve the collection of motion signals from various parts of the human body. Additionally, we explored potential applications of these sensors in fields such as health monitoring and virtual reality. In summary, this work integrated the acquisition of different human motion signals, demonstrating great potential for future multifunctional wearable electronic devices.

Stretchable Sensor Materials Applicable to Radiofrequency Coil Design in Magnetic Resonance Imaging: A Review.

Wearable sensors are rapidly gaining influence in the diagnostics, monitoring, and treatment of disease, thereby improving patient outcomes. In this review, we aim to explore how these advances can be applied to magnetic resonance imaging (MRI). We begin by (i) introducing limitations in current flexible/stretchable RF coils and then move to the broader field of flexible sensor technology to identify translatable technologies. To this goal, we discuss (ii) emerging materials currently used for sensor substrates, (iii) stretchable conductive materials, (iv) pairing and matching of conductors with substrates, and (v) implementation of lumped elements such as capacitors. Applicable (vi) fabrication methods are presented, and the review concludes with a brief commentary on (vii) the implementation of the discussed sensor technologies in MRI coil applications. The main takeaway of our research is that a large body of work has led to exciting new sensor innovations allowing for stretchable wearables, but further exploration of materials and manufacturing techniques remains necessary, especially when applied to MRI diagnostics.

On-demand drug delivery bioelectronics through a water-processable low dimensional highly conductive MXene layer.

On-demand drug delivery holds great promise to optimize pharmaceutical efficacy while minimizing the side effects. However, existing on-demand drug delivery systems often require complicated manufacturing processes that preclude their wide implementation of a broad range of drugs. In this work, we demonstrate the introduction of MXene-coated microneedles (MNs) into bioelectronics for digitally controllable gate-valve drug delivery. MXenes, featuring high electronic conductivity, excellent biocompatibility, and solution processibility, enable low-cost scalability for printable bioelectronics. In an electrolytic state (e.g., body fluid), the coated MXene is oxidized and desorbed due to redox reactions caused by electrical bias, allowing the underlying drug to be controllably released. The MXene-incorporated drug delivery system not only demonstrates excellent biocompatibility and operational stability, but also features low-cost construction and sustainable usage. Besides, these MXene-coated MNs allow both on-demand transformation and local-region customization, further increasing the structural versatility and capability of multidrug delivery systems.

Biocompatible and Biodegradable 3D Graphene/Collagen Fiber Hybrids for High-Performance Conductive Networks and Sensors.

Polymer-based flexible conductive materials are crucial for wearable electronics, electronic skin, and other smart materials. However, their development and commercial applications have been hampered by the lack of strain tolerance in the conductive network, poor bonding with polymers, discomfort during wear, and a lack of biocompatibility. This study utilized oil-tanned leather with a natural network structure, high toughness, and high tensile deformation recovery as a structural template. A graphene (Gr) conductive network was then constructed on the collagen network of the leather, with coordination cross-linking between Gr and collagen fibers through aluminum ions (Al3+). A new flexible conductive material (Al-GL) was then constructed. Molecular dynamics simulations and experimental validation revealed the existence of physical adsorption, hydrogen bonding adsorption, and ligand bonding between Al3+, Gr, and collagen fibers. Although we established that the binding sites between Al3+ and collagen fibers were primarily on carboxyl groups (-COOH), the mechanism of chemical bonding between Gr and collagen fibers remains unclear. The Al-GL composite exhibited a high shrinkage temperature (67.4 °C) and low electrical resistance (16.1 kΩ·sq-1), as well as good softness (9.33 mN), biocompatibility, biodegradability (<60 h), and air and moisture permeability. Furthermore, the incorporation of Al3+ resulted in a heightened Gr binding strength on Al-GL, and the resistance remained comparable following 1 h of water washing. The Al-GL sensor prepared by WPU encapsulation not only demonstrated highly sensitive responses to diverse motion signals of the human body but also retained a certain degree of response to external mechanical effects underwater. Additionally, the Al-GL-based triboelectric nanogenerator (Al-GL TENG) exhibited distinct response signals to different materials. The Al-GL prepared by the one-pot method proposed in this study offers a novel approach to combining functional nanofillers and substrate materials, providing a theoretical foundation for collagen fiber-based flexible conductive materials.

Preparation of Conductive Cellulose Coated with Conductive Polymer and Its Application in the Detection of pH and Characteristic Substances in Sweat.

Rich biological information in sweat provides great potential for health monitoring and management. However, due to the complexity of sweat, the development of environmentally friendly green electronic products is of great significance to the construction of ecological civilization. This study utilized a simple combination of polystyrene sulfonate sodium (PSS) and filter paper (FP) to prepare cellulose materials coated with conductive polymers, developing an electrochemical sensor based on the modified materials. The mechanical and electrochemical properties of the fabricated PSS/FP membrane were optimized by adjusting the feeding dosage of PSS. The realized PSS/FP composite containing 7% PSS displayed good conductivity (9.1 × 10-2 S/m), reducing electric resistance by 99.2% compared with the original FP membrane (6.7 × 10-4 S/m). The stable current of the membrane in simulated sweat under different pH environments is highly correlated with the pH values. Additionally, when the membrane is exposed to simulated sweat with varying ion concentrations, the current signal changes in real time with the concentration variations. The response time averages around 0.3 s.

Collagen fiber-reinforced, tough and adaptive conductive organohydrogel e-skin for multimodal sensing applications.

Conductive hydrogels (CHs) with high sensitivity and multifunctional property are considered as excellent materials for wearable devices and flexible electronics. Surface synapses and internal multilayered structures are key factors for highly sensitive pressure sensors. Nevertheless, current CHs lack environmental adaptability, multifunctional perception, and instrument portability, which seriously hinders their application as sensors. Here, waste collagen fibers (buffing dust of leather), polyvinyl alcohol (PVA) and gelatin (Gel) were used as the basic framework of the hydrogel, loaded with a conductive material (silver nanoparticles (BD-CQDs@AgNPs)) and an anti-freezing moisturizer (glycerol (Gly)), resulting in a multifunctional conductive organohydrogel (BPGC-Gly). As a temperature and humidity sensor, it demonstrated an excellent temperature response range (-20-60 °C) and was capable of rapid response (2.4 s) and recovery (1.6 s) to human breathing. As a strain/pressure sensor, it allowed real-time monitoring of human movement and had a high low-pressure sensitivity (S = 4.26 kPa-1, 0-12.5 kPa). Interestingly, BPGC-Gly could also be used as a portable bioelectrode or the acquisition, monitoring and analysis of EMG/ECG signals. In this work, BPGC-Gly was assembled with wireless transmission to achieve multimodal heath detection, which opens new avenues for multi-responsive CHs, comprehensive human health monitoring and next-generation wearable electronic skin (e-skin).

Carboxymethyl chitosan composited poly(ethylene oxide) electrolyte with high ion conductivity and interfacial stability for lithium metal batteries.

Low ionic conductivity and poor interface stability of poly(ethylene oxide) (PEO) restrict the practical application as polymeric electrolyte films to prepare solid-state lithium (Li) metal batteries. In this work, biomass-based carboxymethyl chitosan (CMCS) is designed and developed as organic fillers into PEO matrix to form composite electrolytes (PEO@CMCS). Carboxymethyl groups of CMCS fillers can promote the decomposition of Lithium bis(trifluoromethane sulfonimide) (LiTFSI) to generate more lithium fluoride (LiF) at CMCS/PEO interface, which not only forms ionic conductive network to promote the rapid transfer of Li+ but also effectively enhances the interface stability between polymeric electrolyte and Li metal. The enrichment of carboxyl, hydroxyl, and amidogen functional groups within CMCS fillers can form hydrogen bonds with ethylene oxide (EO) chains to improve the tensile properties of PEO-based electrolyte. In addition, the high hardness of CMCS additives can also strengthen mechanical properties of PEO-based electrolyte to resist penetration of Li dendrites. LiLi symmetric batteries can achieve stable cycle for 2500 h and lithium iron phosphate full batteries can maintain 135.5 mAh g-1 after 400 cycles. This work provides a strategy for the enhancement of ion conductivity and interface stability of PEO-based electrolyte, as well as realizes the resource utilization of biomass-based CMCS.

On the design of lignin reinforced acrylic acid/hyaluronic acid adhesive hydrogels with conductive PEDOT:HA nanoparticles.

Hydrogels are of great importance in biomedical engineering. They possess the ability to mimic bodily soft tissues, and this allows exciting possibilities for applications such as tissue engineering, drug delivery and wound healing, however much work remains on stability and mechanical robustness to allow for translation to clinical applications. The work herein describes the synthesis and analysis of a biocompatible, versatile hydrogel that has tailorable swelling, high stability when swollen and thermal stability. The synthesis methods used produce a hydrogel with high elasticity, good mechanical properties and rapid crosslinking whilst displaying biocompatibility, adhesion, and conductivity. It has been shown that cell viability in the samples is above 80 % in all cases, a Young's Modulus of up to 85 kPa and high swelling degrees were achieved. These materials show potential for use in numerous applications such as adhesive sensors, skin grafts and drug delivery systems.

Spectroscopic investigation, dielectric and antimicrobial properties of chitin-cellulose@ZnO/CuO conductive nanocomposites.

In this research, we fabricated a functional conductive nanocomposite with valuable properties through a chitin (CH) and cellulose (CE) polymerization process, incorporating ZnO/(0.1, 0.2, 0.3 mol.%) CuO bioactive nanoparticles. These bioactive nanoparticles, synthesized through sol-gel and polymerization interactions, greatly enhanced the structural, dielectric, and antimicrobial characteristics of CH-CE@ZnO/CuO conductive nanocomposites. The morphological analysis revealed that these nanoparticles, with diameters ranging from 11-25 nm, formed covalent bonds with the membrane matrix, bolstering the conductive nanocomposites ' structural integrity and dielectric performance. The dielectric properties of the conductive nanocomposites were significantly enhanced by the even distribution of ZnO/CuO nanoparticles within the CH-CE composite. Additionally, antimicrobial assessments demonstrated that the CH-CE@ZnO/CuO conductive nanocomposites displayed significant antibacterial properties against the Escherichia coli and Staphylococcus aureus, showcasing their potential as active packaging materials for electronic, biosensors, and sustainable applications.

Continuous dual-network alginate hydrogel fibers with superior mechanical and electrical performance for flexible multi-functional sensors.

Hydrogel fibers play a crucial role in the design and manufacturing of flexible electronic devices. However, continuous production of hydrogel fibers with high strength, toughness, and conductivity remains a significant challenge. In this study, ion-conductive sodium alginate/polyvinyl alcohol composite hydrogel fibers with an interlocked dual network structure were prepared through continuous wet spinning based on the pH-responsive dynamic borate ester bonds. Owing to the interlocked dual network structure, the resulting hydrogel fibers integrated superior performance of strength (4.31 MPa), elongation-at-break (>1500 %), ion conductivity (17.98 S m-1) and response sensitivity to strain (GF = 3.051). Benefiting from the excellent performance, the composite hydrogel fiber could be applied as motion-detecting sensors, including high-frequency, high-speed reciprocating mechanical motion, and human motion. Furthermore, the superior compatibility for human-computer interaction of the hydrogel fiber was also demonstrated, which a manipulator could be controlled to perform different actions, by a smart glove equipped with the hydrogel fiber sensors.

Plasticised chitosan: Dextran polymer blend electrolyte for energy harvesting application: Tuning the ion transport and EDLC charge storage capacity through TiO2 dispersion.

This study investigates the performance of biopolymer electrolytes based on chitosan and dextran for energy storage applications. The optimization of ion transport and performance of electric double-layer capacitors EDCL using these electrolytes, incorporating different concentrations of glycerol as a plasticizer and TiO2 as nanoparticles, is explored. Impedance measurements indicate a notable reduction in charge transfer resistance with the addition of TiO2. DC conductivity estimates from AC spectra plateau regions reach up to 5.6 × 10-4 S/cm. The electric bulk resistance Rb obtained from the Nyquist plots exhibits a substantial decrease with increasing plasticizer concentration, further enhanced by the addition of the nanoparticles. Specifically, Rb decreases from ∼20 kΩ to 287 Ω when glycerol concentration increases from 10 % to 40 % and further drops to 30 Ω with the introduction of TiO2. Specific capacitance obtained from cyclic voltammetry shows a notable increase as the scan rate decreases, indicating improved efficiency and stability of ion transport. The TiO2-enriched EDCL achieves 12.3 F/g specific capacitance at 20 mV/s scan rate, with high ion conductivity and extended electrochemical stability. These results suggest the great potential of plasticizer and TiO2 with biopolymers in improving the performance of energy storage systems.

Biopolymer electrolyte from banana powder-konjac glucomannan for zinc-ion batteries.

Herein, the novel eco-friendly biopolymer electrolytes consisting of banana powder and konjac glucomannan host matrix doped with zinc acetate salt were successfully fabricated through simple casting technique. The biopolymer electrolyte exhibited satisfactory thermal stability and mechanical properties; tensile strength (13.82 MPa); elongation at break (60.52 %) and Young's modulus (93.2 MPa). The electrochemical studies were carried out in symmetrical cells Zn/Zn cells. Biopolymer electrolyte showed favorable ionic conductivity of 5.59 × 10-4 S/cm along with stable cycling performance. The potential stability was found to be 2.52 V. The as-prepared biopolymer electrolytes demonstrated the potential as green, simple yet effective biopolymer electrolytes for zinc-ion batteries.

Development of lignin hydrogel reinforced polypyrrole rich electrode material for supercapacitor and sensing applications.

The preparation of natural polymer-based highly conductive hydrogels with reliable durability for applications in supercapacitors (SCs) is still challenging. Herein, a facile method to prepare alkaline lignin (AL)-based polypyrrole (PPy)-rich, high-conductive PPy@AL/PEGDGE gel was reported, where AL was used as a dopant, polyethylene glycol diglycidyl ether (PEGDGE) as a cross-linking agent, and PPy as a conducting polymer. The PPy@AL/PEGDGE gel electrode materials with hollow structures were prepared by electrochemical deposition and chemical etching method and then assembled into sandwich-shaped SCs. Cyclic voltammetry (CV), galvanotactic charge discharge (GCD), electrochemical impedance spectroscopy (EIS) and cycling stability tests of the PPy@AL/PEGDGE SCs were performed. The results demonstrated that the SCs can achieve a conductivity of 25.9 S·m-1 and a specific capacitance of 175 F·g-1, which was 127.4 % higher compared to pure PPy (77 F·g-1) electrode. The highest energy density and power density for the SCs were obtained at 23.06 Wh·kg-1 and 5376 W·kg-1, respectively. In addition, the cycling performance was also higher than that of pure PPy assembled SCs (50 %), and the capacitance retention rate can reach 72.3 % after 1000 cycles. The electrode materials are expected to be used as sensor and SCs devices.